College of Biology and the Environment, Nanjing Forestry University, Nanjing, 210037, Jiangsu, People's Republic of China.
College of Biology and the Environment, Nanjing Forestry University, Nanjing, 210037, Jiangsu, People's Republic of China.
Water Res. 2021 Jun 15;198:117143. doi: 10.1016/j.watres.2021.117143. Epub 2021 Apr 15.
UV/sulfite systems with oxygen have recently been considered as advanced oxidation processes in view of the participation of oxysulfur radicals. However, the contribution of •OH and the efficiency of destructing emerging contaminants (ECs) in water remain largely unclear. Here, the UV/S(IV) process was applied with natural reoxygenation to degrade two typical ECs, diethyl phthalate (DEP) and bisphenol A (BPA) showing different properties. Solution pH played the key role in determining the reactive species, and both DEP and BPA were more favorably degraded at more alkaline conditions with higher utilization efficiency of SO. Specifically, the H•, O, •OH and SO were identified at acidic condition, but the amount of •OH accumulated significantly with the elevation of pH. Competitive quenching experiments showed that e and •OH dominated the degradation of DEP and BPA at alkaline condition, respectively. Besides, DEP showed higher quantum efficiency for the indirect photolysis and mineralization degree than that of BPA at pH 9.2 mainly due to the direct use of the primary photoproduct. The possible transformation mechanisms of S(IV) and mineralization routes of both pollutants were proposed. This study may provide new insights into the mechanisms involved in UV/S(IV) process and a promising alternative for efficient removal of ECs in water.
UV/sulfite 体系与氧气结合,由于氧硫自由基的参与,最近被认为是一种高级氧化工艺。然而,羟基自由基的贡献和水中新兴污染物(ECs)的破坏效率在很大程度上仍不清楚。本研究采用自然复氧的 UV/S(IV) 工艺来降解两种典型的 ECs,邻苯二甲酸二乙酯(DEP)和双酚 A(BPA),它们具有不同的性质。溶液 pH 值在确定反应性物种方面起着关键作用,DEP 和 BPA 在碱性条件下更有利于降解,SO 的利用率更高。具体而言,在酸性条件下鉴定出 H•、O、•OH 和 SO,但随着 pH 值的升高,•OH 的积累量显著增加。竞争猝灭实验表明,在碱性条件下,e 和•OH 分别主导 DEP 和 BPA 的降解。此外,由于直接利用初始光产物,在 pH 9.2 时,DEP 的间接光解量子效率和矿化程度均高于 BPA。提出了 S(IV)的可能转化机制和两种污染物的矿化途径。本研究可为 UV/S(IV) 工艺的机制提供新的见解,并为水中有效去除 ECs 提供一种有前景的替代方法。